期刊
ADVANCED ENERGY MATERIALS
卷 9, 期 14, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/aenm.201803935
关键词
ambient temperature ammonia production; electrocatalytic nitrogen reduction; inhibition of HER activity; Li-S interactions; MoS2 nanosheets
类别
资金
- National Natural Science Foundation of China [51432009, 51672277]
- CAS Pioneer Hundred Talents Program
- CAS/SAFEA International Partnership Program for Creative Research Teams of Chinese Academy of Sciences, China
The Haber-Bosch process can be replaced by the ambient electrocatalytic N-2 reduction reaction (NRR) to produce NH3 if suitable electrocatalysts can be developed. However, to develop high performance N-2 fixation electrocatalysts, a key issue to be resolved is to achieve efficient hydrogenation of N-2 without interference by the thermodynamically favored hydrogen evolution reaction (HER). Herein, in-operando created strong Li-S interactions are reported to empower the S-rich MoS2 nanosheets with superior NRR catalytic activity and HER suppression ability. The Li+ interactions with S-edge sites of MoS2 can effectively suppress hydrogen evolution reaction by reducing H* adsorption free energy from 0.03 to 0.47 eV, facilitate N-2 adsorption by increasing N-2 adsorption free energy from -0.32 to -0.70 eV and enhance electrocatalytic N-2 reduction activity by decreasing the activation energy barrier of the reaction control step (*N-2 *N2H) from 0.84 to 0.42 eV. A NH3 yield rate of 43.4 g h(-1) mg(-1) MoS2 with a faradaic efficiency (FE) of 9.81% can be achieved in presence of strong Li-S interactions, more than 8 and 18 times by the same electrocatalyst in the absence of Li-S interactions. This report opens a new way to design and develop catalysts and catalysis systems.
作者
我是这篇论文的作者
点击您的名字以认领此论文并将其添加到您的个人资料中。
推荐
暂无数据